The hydrogenation activity of noble metal, especially platinum (Pt), catalysts can be easily inhibited by the presence of a trace amount of carbon monoxide (CO) in the reaction feeds. Developing CO-resistant hydrogenation catalysts with both high activity and selectivity is of great economic interest for industry as it allows the use of cheap crude hydrogen and avoids costly product separation. Here we show that atomically dispersed Pt over α-molybdenum carbide (α-MoC) constitutes a highly CO-resistant catalyst for the chemoselective hydrogenation of nitrobenzene derivatives. The Pt1/α-MoC catalyst shows promising activity in the presence of 5,000 ppm CO, and has a strong chemospecificity towards the hydrogenation of nitro groups. With the assistance of water, high hydrogenation activity can also be achieved using CO and water as a hydrogen source, without sacrificing selectivity and stability. The weakened CO binding over the electron-deficient Pt single atom and a new reaction pathway for nitro group hydrogenation confer high CO resistivity and chemoselectivity on the catalyst.
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The data that support the plots within this paper and other findings of this study are available from the corresponding author, X.D.W., upon reasonable request.
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This work was financially supported by the Natural Science Foundation of China (21725301, 91645115, 21872104, 21473003, 51622211, 21473229 and 91545121) and the National Key R&D Program of China (2017YFB0602200). The electron microscopy work performed in the CAS Key Laboratory of Vacuum Sciences was supported in part by the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (CAS) and the Pioneer Hundred Talents Program of the CAS. The XAFS experiments were conducted at the Shanghai Synchrotron Radiation Facility. The authors also acknowledge the innovation foundation of the Institute of Coal Chemistry, CAS, the Hundred-Talent Program of the CAS, the Shanxi Hundred-Talent Program and the National Thousand Young Talents Program of China. The scholarship under the International Postdoctoral Exchange Fellowship Program 2017 by the Office of China Postdoctoral Council (document 496 number: no. 32 Document of OCPC, 2017) is also gratefully acknowledged. The authors also appreciate B. Qiao for discussions and for providing the Pt1/FeOx single atom catalyst as a reference.
The authors declare no competing interests.
Journal peer review information: Nature Nanotechnology thanks Nigel Powell, Yung-Eun Sung and other anonymous reviewer(s) for their contribution to the peer review of this work.
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Lin, L., Yao, S., Gao, R. et al. A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation. Nat. Nanotechnol. 14, 354–361 (2019). https://doi.org/10.1038/s41565-019-0366-5
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